The First Mixed Valence Radical Cation Salts of BEDT-TTF with the Photochromic Metal Mononitrosyl Complexes [RuNOX5]2- (X=Br, Cl) as Counterions

New molecular complexes of fullerenes C60 and C70 with leuco crystal violet (LCV, 1 -3); leucomalachite green (LMG, 4-6); crystal violet lactone (CVL, 7); N,N,Nʹ,Nʹ-tetrabenzyl-p-phenylenediamine (TBPDA, 8, and 9); N,N,Nʹ,Nʹ-tetramethyl-pphenylenediamine (TMPDA, 10, and 11); triphenylamine (TPA, 12, and 13); and substituted phenotellurazines (EPTA and TMPTA, 14, and 15) have been synthesized. Crystal structures have been solved for C60 complexes with LMG (5, 6) TBPDA (8), TMPDA (10), and TPA (12). The C60 molecules form closely packed double layers in 5 and 6, hexagonal layers in 10 and quasi-three-dimensional layers in 8 and 12. The substitution of disordered solvent molecules in the complexes with LMG (4, 5) by naphthalene ones results in the ordering of the C60 molecules. According to IR-, UV-visible-NIR and ESR-spectroscopy the complexes have a neutral ground state. The spectra of 1-8, and 10 show intense charge transfer bands in the visible and NIR-range. On photoexcitation by white light (lightinduced ESR (LESR) spectroscopy), 1 and 10 were shown to have an excited ionic state. The LESR signals were generated at light energies <2.25 eV indicating that the excited states in the complexes are realized mainly by direct charge transfer from donor to the C60 molecule.